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International Journal of Food Properties

ISSN: 1094-2912 (Print) 1532-2386 (Online) Journal homepage: https://www.tandfonline.com/loi/ljfp20

Comparison of crystallized coconut sugar


produced by traditional method and amorphous
coconut sugar formed by two drying methods:
vacuum drying and spray drying

Bambang Nurhadi, Nandi Sukri, Wahyu Kristian Sugandi, Annisa Puteri


Widanti, Resi Restiani, Ziske Noflianrini, Bayu Rezaharsamto & Marleen
Herudiyanto

To cite this article: Bambang Nurhadi, Nandi Sukri, Wahyu Kristian Sugandi, Annisa Puteri
Widanti, Resi Restiani, Ziske Noflianrini, Bayu Rezaharsamto & Marleen Herudiyanto (2018)
Comparison of crystallized coconut sugar produced by traditional method and amorphous coconut
sugar formed by two drying methods: vacuum drying and spray drying, International Journal of
Food Properties, 21:1, 2339-2354, DOI: 10.1080/10942912.2018.1517781

To link to this article: https://doi.org/10.1080/10942912.2018.1517781

© 2018 The Author(s). Published by Taylor &


Francis.

Published online: 24 Sep 2018.

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INTERNATIONAL JOURNAL OF FOOD PROPERTIES
2018, VOL. 21, NO. 1, 2339–2354
https://doi.org/10.1080/10942912.2018.1517781

Comparison of crystallized coconut sugar produced by traditional


method and amorphous coconut sugar formed by two drying
methods: vacuum drying and spray drying
Bambang Nurhadi, Nandi Sukri, Wahyu Kristian Sugandi, Annisa Puteri Widanti, Resi Restiani,
Ziske Noflianrini, Bayu Rezaharsamto, and Marleen Herudiyanto
Faculty of Agric. Industrial Technology, Universitas Padjadjaran, Sumedang, Indonesia

ABSTRACT ARTICLE HISTORY


Coconut sugar is traditionally produced by evaporating sap until reaching its Received 5 June 2018
saturated liquid and formed a crystalline structure. This study investigated the Accepted 27 August 2018
comparison of coconut sugar made by traditional method (crystalline struc-
KEYWORDS
ture) and dried coconut sugar (predominantly amorphous structure) to its Coconut sugar powder;
characteristics. Two different formulation of coconut sap : maltodextrin (7 : 3) maltodextrin; spray drying;
and (6 : 4) (weight/weight) were dried using vacuum oven (70℃, 6 hours) and vacuum drying; Amorphous
spray dried (Tinlet 120℃.) Coconut sugar was characterized for moisture con- and Crystalline structure
tent, crystallinity, water sorption isotherm, hygroscopic rate, color, dissolving
time, and powder recovery. Initial moisture content was examined and in
range of 1.33% - 3.44% (wb). The highest monolayer water content was
obtained by using spray drying (6 : 4) and lowest was obtained by traditional
method. X-ray diffraction showed that dried coconut sugar powder had domi-
nant amorphous structure (70.9 – 71.4%) while traditional one was dominated
with crystalline structure (90.5%). Traditional coconut sugar was the least
hygroscopic (1.21 × 10-4 g water/g solid/minutes), followed by vacuum dried
coconut sugar (1.48 × 10-4 g water/g solid/minutes) and spray dried ones (1.56
– 1.67 × 10-4 g water/g solid/minutes). Spray dried coconut sugar had the
brightest and the whitest color, followed by vacuum dried and traditional
coconut sugar. Vacuum dried powder was quicker to dissolve (13.33 – 16.67
s), while increasing maltodextrin in spray drying could not decrease the
dissolving time. The highest powder recovery of dried sugar was obtained by
using vacuum drying and higher maltodextrin concentration (88.70%) while
traditional method produced 100% powder recovery.

Introduction
Traditional coconut sugar powder in Indonesia is made by heating coconut sap until reaching its
saturated solution and continued to heat into crystallized-structured sugar 1 This method is based on
co-crystallization principle. There are two types of coconut sugar, firstly granulated coconut sugar
which is produced by continued heating the supersaturated coconut sap until crystallized structure
appeared. Secondly, the supersaturated coconut sap is put in a special container and cooled to
produce a certain shaped form of coconut sugar.
The drying of coconut sap into coconut sugar powder is difficult to accomplish as it is
composed of mostly sucrose (12.30–17.40%) 2 and corresponding to the problem of stickiness
while drying. One of the factors contributing to stickiness is low glass transition temperature
(Tg). Tg is a change observed when a glassy state is turning into a super-cooled melt during
heating 3, while sucrose has Tg of 62°C and considered low when it comes to drying 4 To

CONTACT Bambang Nurhadi bnhnur@gmail.com


Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/ljfp.
© 2018 The Author(s). Published by Taylor & Francis.
This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/), which
permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
2340 B. NURHADI ET AL.

overcome this problem, the glass transition temperature of the coconut sap can be increased by
the addition of a coating material having a higher glass transition temperature than sucrose.
Maltodextrin (MD) is a carbohydrate derivative mostly used as drying aid of high sugar material
5
Glass transition temperature of MD depends on dextrose equivalent (DE) value, often in range
of 140–180°C6 MD with DE 10 with Tg of 112°C is considered a better material to maintain
stability compared to other materials such as trehalose 7 MD may also increase process stability
and storage of solid food to reduce caking, stickiness, and increasing ability to flow 8 Addition of
MD ≥ 50% (solid/solid, w/w)) is needed to create a significant impact on glass transition
temperature.[9,10]
Despite the use of high molecular material, in order to successfully dry high sugar material,
the rate of drying process should be high 5 This can be accomplished by vacuum drying and
spray drying method. Vacuum drying is a process in which the material is dried in a low-
pressure environment, which lowers the heat required for rapid drying 11 Based on ideal gas
law, at low absolute pressure (vacuum conditions), water can evaporate at a lower tempera-
ture than normal conditions (ambient pressure, 1 atm). This causes drying to occur more
rapidly at lower temperatures 5 Similar high sugar content food, mango powder and honey
powder, was successfully dried by adding MD as drying aid using vacuum oven at 70°C.[12,]
Spray drying is a method to produce dry and fine particles with atomization process of
samples into small droplets in a hot air environment. Due to its large surface area and high
temperature, the droplets would dry quickly and hence fall to lower part of the dryer.13 Coconut
sugar powder was successfully dried using a spray dryer with inlet temperatures of (120°C, 150°
C, and 180°C), and the concentrations of MD (DE 9–12) used were 10%, 20%, and 30% (weight/
volume). The optimum condition of producing coconut sugar powder with good appearance and
solubility parameters is MD concentration of 20% (w/v) and inlet temperature of 120°C.14 The
aim of the recent work was to compare the properties of coconut sugar produced from two
different methods, traditional (co-crystallization) and drying method. The observed properties
were moisture content, water sorption isotherm, amorphous content, hygroscopic rate, colour,
dissolving time, and powder recovery. This work also compared the coconut sugar powder
properties produced by vacuum drying and spray drying method.

Materials and method


Materials
Coconut sap was obtained freshly from Kertamukti village, Pangandaran District, West Java,
Indonesia (±170 km from the lab). Coconut sap was collected from coconut flower and lime
(mainly content Ca(OH)2) was previously added to maintain the pH (8.8) and then boiled in a
cauldron for 1 h to reduce microorganisms and the process was done in a farmer’s house. Pre-
boiled coconut sap was put in containers and kept in low temperature (10–15°C) during the
travel for 4–5 h using an ice box and taken to the laboratory, Department of Food Industrial
Technology, Faculty of Agroindustrial Technology, University of Padjadajaran, Jatinangor,
Indonesia. Coconut sap was kept frozen (GEA Chest Freezer, China) at −28°C during prepara-
tion and only being thawed in room temperature before being used in further experiments.
Maltodextrin DE 13–15 (Lihua Starch, China) was used as drying aid. The chemicals in this
study include CH3COOK, MgCl2, K2CO3, Mg(NO3)2, NaNO2, and NaCl (Merck, Germany) for
water sorption isotherm experiment. Silica gel and aquades were also used to complete the
experiment.
INTERNATIONAL JOURNAL OF FOOD PROPERTIES 2341

Coconut sugar powder production


Traditional method
Coconut sap was poured in a hot pan and continuous stirring was done in 90–100°C using a spatula.
As the coconut sap turned into a viscous liquid, heat was reduced while stirring continued until
granules were formed.15 Sample was cooled before grinding. The powder obtained from grinding
step then was put in a heat-sealed plastic and then kept in a desiccator before further analysis.

Drying methods
Coconut sap was tested by using a refractometer to observe dissolved solid (°Brix). Maltodextrin
(MD) DE 13–15 (5.0% moisture content) was added with ratio of coconut sap (C) : maltodextrin
(MD) of 7 : 3 and 6:4 (solid to solid) accordingly. Distilled water was added to adjust the total solid
content of the solution to 20°Brix. Then, it was added to coconut sap directly using a magnetic stirrer
to create a homogenous solution.

Vacuum drying
Vacuum oven (Binder VD 23, Tuttington, German) was used to perform the drying process. Samples
are put into a silicone container with thickness of ±1.5 cm. The temperature of vacuum oven was set
to 70°C with absolute pressure of 5 inHg and drying time of 56 h 12 After drying was completed,
samples were put into desiccator to decrease the temperature into ambient temperature. After
grinding, the powder was put in a heat-sealed plastic then kept in a desiccator before further analysis.

Spray drying
Spray drying was performed using a pilot scale spray dryer (Kodi Machinery LPG-5, Jiangsu, China)
using co-current flow. Inlet temperature of 120°C and outlet temperature of 65°C and flow rate of
8.0 rpm were maintained during the drying.14 The resultingpowder was then packed in a heat-sealed
plastic bag and was kept in a desiccator before further analysis was performed.

Sugar content
Sugar content of fresh coconut sap was determined by using High Performance Liquid Chromatography
(HPLC) method by using carbohydrate column (4.6 mm × 250 mm), particle size 4µm, mobile phase:
Acetonitril–Aquabidest (80:20) (volume/volume), velocity of mobile phase 2.0 mL/min with refractive
index detector, and column temperature of 40°C:16
Area
Slope  Final VolumeðmlÞ  Dillution Factor
% Sugar content ¼ (1)
gsample

Moisture content
Moisture content of coconut sugar powder was estimated by using gravimetric method. The
gravimetric method, based on water removal by heating, was carried out in a convective oven at
105°C ± 5°C for 6 h.16

Water sorption isotherm


Water sorption isotherm was determined by using gravimetric method. Six saturated salt solutions
were prepared (CH3COOK, MgCl2, K2CO3, Mg(NO3)2, NaNO2, and NaCl) in order to provide
relative humidity values of 22.6%, 32.73%, 43.80%, 52.86%, 68.9%, and 75.32%, respectively.
Triplicate samples of 1 g of coconut sugar powder were weighed into vials and equilibrated over
such saturated solutions, in desiccators at 25°C. The equilibrium is reached when the weight of the
2342 B. NURHADI ET AL.

sample did not exceed 0.001 g change.17 The Guggenheim, Anderson, and de Boer (GAB) (Eq. 2)
and Brunauer, Emmet, and Teller (BET) (Eq. 3) models were used to define the relationship of
equilibrium moisture content to water activity.
Xm CKaw
X¼ (2)
ð1  Kaw Þð1 þ ðC  1ÞKaw Þ
Xm Caw
X¼ (3)
ð1  aw Þð1 þ ðC  1Þaw Þ
X = Moisture content (g water/g dry solid)
aw = Water activity
Xm = Monolayer water content
Xm, C, and K are constants.
The goodness of fit of the model was described by mean relative deviation (MRD):
 
1 Xe  Xp
MRD ¼ abs (4)
n Xe
where Xe is moisture content obtained from observation; Xp is predicted equilibrium moisture
content (dry basis) calculated from different models; n is the number of data points. MRD <5
indicates best fit for the sample, while 5 < MRD < 10 indicates good fit, while MRD >10 indicates
unsuitable fit of the model used.18

X-ray diffraction
X-ray diffraction analysis (XRD D8 Advance A25 Bruker, Germany) was conducted to determine the
structure of coconut sugar powder, i.e., crystalline or amorphous structure. The amorphous and
crystalline structure percentage was also determined by using software provided in the equipment.

Hygroscopic rate measurement


Hygroscopic rate was measured by determining the slope of weight change of sample during storage
at Relative Humidity (RH) 75% while collecting samples' weight in certain interval for 4 h. 19

Colour analysis
Spectrophotometer (Konica Minolta CM-5 Sensing Singapore Pte Ltd) was used to examine the
colour characteristics. The results were expressed as L*, a*, and b*. L* value determines lightness or
darkness, a* determine redness or greenness, while b* determines yellowness or blueness.20

Dissolving time
Dissolving time is determined by measuring the time for the powder to completely dissolved in
water. One gram of the sample is dissolved by pouring into 50 ml of water. Magnetic stirrer was used
to create a homogenous solution.21

Powder recovery
22
Powder recovery was analysed by comparing powder yield to its original solid content in dry

Yieldð g Þ
Powder Recovery ¼  100%
Initial weight of solids in solutionð g Þ
INTERNATIONAL JOURNAL OF FOOD PROPERTIES 2343

Results and discussion


Coconut sap properties
Coconut sap is a nutritious material due to its composition and easily fermented and deteriorated
during collection. Traditionally, the farmers usually add preservative (natural or chemical preserva-
tive) and lime (Ca(OH)2) to maintain the stability of coconut sap during further processing.
Properties of fresh coconut sap are shown in Table 1. pH of coconut sap is in neutral range 23,
while pH of coconut sugar was 6.00–7.78 when lime (Ca(OH)2) was added.24 Similar result is shown
by the data above that pH of coconut sugar with added lime (Ca(OH)2) is about 7.47 ± 0.04. Water
activity of coconut sap is 1.00, which indicates a high-moisture food. Food that contains water
activity of 0.90–0.999 contains more than 50% (w/w) water 25
From Table 1, it is known the total soluble solid of coconut sap is about 20.70°Brix. It means that
total solid in coconut sap is about 20% of total solution. Solids in coconut sap consist of sugar such
as sucrose 85.76% (s/s), fructose 1.5% (s/s), and glucose <0.82% (s/s). The sucrose content was
slightly higher (Table 1) than was reported by Kalaiyarasi et al.26 where fresh coconut sap had
12–15% of sucrose (by weight) and some reducing sugar, such as glucose, fructose, maltose, and
raffinose. Sucrose contents of coconut sap varied from 9.40 to 12.24 g/100 ml, from 1.63 to1.84 g/
100ml glucose content, while fructose constituted from 1.24 to 1.52 g from 100 ml of sap.27 Study
reports that coconut sap had rapid fermentation, unless it is collected under hygiene condition,
and sugar still can be transformed into alcohol (5–8%).28 This fact might explain the lower content
of glucose compared to fructose of the coconut sap sample (Table 1).
Colour of coconut sap is valued by L*, a*, and b*. Positive L* value means coconut sap tends to
show a brighter colour, a* and b* values are also positive means coconut sap tends to show red and
yellow colours. It is caused by the Maillard reaction. Before coconut sap was taken to the laboratory
for the experiment, it had been cooked for several hours until boiled, so that it might cause
the Maillard reaction to take place that accentuated the red and yellow colours of the coconut sap.

Moisture content
The moisture content of coconut sugar powder is presented in Table 2 in the range of 1.33–3.44%.
Moisture content of traditional coconut sugar powder is in agreement with Zuliana29, which is 1.37–
2.43%. Similar results were found in drying of apple juice using vacuum drying and spray drying
with the addition of maltodextrin with moisture content of 1.1–5.6%30, and drying of honey
powder.[19,]
Addition of maltodextrin as drying aid to coconut sugar powder leads to an increase in moisture
content in both drying methods. This is due to maltodextrin hydrophilic sites, which might bind
more water and affect the moisture content overall 17 Spray-dried coconut sugar powder showed less

Table 1. Properties of coconut sap.


Parameter Value
pH 7.47 ± 0.04
aw 1.00 ± 0.006
Total soluble solid (°Brix) 20.73 ± 0.64
Color
L 72.61 ± 0.37
a 3.18 ± 0.03
b 17.80 ± 0.02
Glucose(%) < 0.17
Fructose(%) 0.32 ± 0.03
Sucrose(%) 17.78 ± 0.06
2344 B. NURHADI ET AL.

Table 2. Moisture content of coconut sugar powder produced by traditional method and drying methods.
Treatments Moisture content (%wb)
Traditional 1.97 ± 0.70
Vacuum dried, C : MD = 7 : 3 1.93 ± 0.16
Vacuum dried, C : MD = 6 : 4 3.40 ± 4.09
Spray dried, C : MD = 7 : 3 1.33 ± 0.07
Spray dried, C : MD = 6 : 4 3.44 ± 0.08

moisture content because of rapid drying and higher surface area due to atomization hence less
moisture content 31

Water sorption isotherm


The water sorption of coconut sugar powder produced by traditional method and drying methods is
presented in Fig. 1 and Fig. 2. The powder which was kept in higher water activity showed longer
time to reach equilibrium while the powder which was kept in lower water activity surrounding. A
slow increase in moisture content at low water activity and steep rise in high water activity is a
typical behaviour for sugar-rich foods, including banana flake.32 Increasing maltodextrin in each
drying method impacted on time to reach the equilibrium state. Both spray drying and vacuum
drying showed the same behaviour at increased maltodextrin concentrations (Fig. 1).
The approach to GAB and BET equation to water sorption values of coconut sugar powder was
performed by using theleast square difference method. The results of both models are shown in
Table 3. The BET model analysis is based on an over-simplified assumption; hence, the model is not
expected to hold for water sorption in foods for a wide range of moisture, but calculation for the
monolayer concept is considered effective for estimating the amount of bound water to specific polar
sites in dehydrated food system.33 While the GAB isotherm equation is the extension of the BET
model, introducing a third parameter, K, which involves the modified properties of the sorbate in the
multilayer region and bulk liquid properties. The GAB model is considered the best fit for food
materials with a wide range of water activity 34
The fitness of the model was analysed by MRD value, where the less the value the better for the
model to fit. MRD <5 indicated best fit for the sample, while 5 < MRD < 10 indicated good fit, while
MRD > 10 indicated unsuitable fit of the model used. As given in Table 3, based on the smallest
value of MRD for each sample, the GAB model gave a better fit to water sorption of dried coconut
sugar powder than BET model. The GAB model also fitted the water sorption isotherms of vacuum-
dried honey powder compared to BET model 10
Xm or the monolayer moisture content indicates the amount of absorbed water to specific sites at
the food surface. To ensure that there is a minimal rate of deteriorative reactions, except for
oxidation of unsaturated fats, the safest water activity level is the one corresponding with Xm or
lower.[35,36] As given in Table 3, the BET monolayer water content of coconut sugar powder is in the
range of 0.025–0.056 g/g. The highest monolayer moisture content is shown by spray dried coconut
sugar powder with the highest maltodextrin content. Similar results were found with vacuum-dried
honey powder 10, freeze-dried papaya pulp powder37, in which increasing maltodextrin resulted in
higher monolayer water content, thus creating a stable honey powder. This is due to the high
molecular weight of maltodextrin, which results in a higher glass transition temperature, giving a
more stable powder at room temperature.
The coconut sugar powder obtained by traditional method showed the least water sorption at each
aw compared to coconut sugar powder from other treatments. This might be due to the predominantly
crystalline structure of traditional coconut sugar powder than those of drying methods. Drying method
commonly produced amorphous structure 38 and semi-crystalline structure. Crystalline material
absorb small amount of water until deliquescence occurs, compared to amorphous structure which
absorbs more water in low water activity.5 After deliquescence point, equilibrium curve in crystalline
INTERNATIONAL JOURNAL OF FOOD PROPERTIES 2345

Figure 1. The increase of coconut sugar powder moisture content exposed to different relative humidities.

will significantly increase.39 Amorphous lactose also absorbed more water in low water activity
compared with crystalline lactose.40 Higher monolayer water content correlated to higher amorphous
content of semi-crystalline lactose powder.41 From Table 3, it is known that the coconut sugar powder
obtained by spray drying method showed the highest monolayer water content, meaning higher
amorphous content than the coconut sugar powder from other treatments. The traditional coconut
sugar which predominantly showed crystalline structure had the least monolayer water content.

X-ray diffraction
The structure of powder particle, whether it is a crystalline or amorphous can be determined by
means of analysis X-ray diffraction. Each dried sample was compared to coconut sugar powder
produced by traditional method. The traditional coconut sugar showed the typical crystalline XRD
pattern and had been confirmed being crystalline sucrose structure. In traditional method, coconut
2346 B. NURHADI ET AL.

Figure 2. The relationship between moisture content and water activity of coconut sugar powder produced by traditional method
and drying methods. The insetshows a zoom picture of low aw.

Table 3. Estimated GAB and BET parameters of coconut sugar powder produced by traditional method and drying methods.
BET model GAB model
Ratio of samples Xm (gg) c Rsq MRD Xm (gg) c k Rsq MRD
Traditional 0.003 11.90 0.60 31.47 0.034 1.00 1.00 0.95 128.78
VD 7 : 3 0.025 3.97 0.74 4.15 0.033 1.589 1.00 0.89 0.27
VD 6 : 4 0.048 2.59 0.94 1.93 0.060 2.781 0.83 0.95 2.14
SD 7 : 3 0.055 1.44 0.92 20.54 0.051 2.636 0.85 0.91 13.62
SD 6 : 4 0.056 5.16 0.91 1.42 0.069 2.145 1.00 0.98 1.18

sap was heated until reaching its saturated liquid, the heat then lowered and continued to stir until
crystallized sugar was formed. The pH of the coconut sap should be neutral (or higher) to avoid
hydrolysis of sucrose during heating that resulting in crystallized structure not formed into glucose
and fructose. Thus, the farmers usually add preservative and lime into coconut sap to make
crystallized sugar in the next process. In drying process (both spray drying and vacuum drying),
the evaporation of water is too quick that might be not enough time for sucrose to crystallize during
drying and consequently less crystalline structure formed. Some crystalline structure was reported in
vacuum-dried honey powder 5 and spray-dried sucrose-lactose powder.42 The result is shown in
Fig. 3.
X-ray diffraction profile between traditional and drying methods showed substantial difference.
Compared to traditional coconut sugar powder, the presence of sharp and defined peaks in crystal-
line materials is due to the fact that the molecules are in an orderly manner while amorphous
material with its disorderly molecules will produce disperse bands and creating wide peak. 43
Maltodextrin incorporated spray-dried mango powder showed similar x-ray diffraction profile 44,
spray-dried coconut sap 45, and spray-dried sucrose powder.46 Amorphous nature of dried coconut
sugar powder is due to rapid evaporation and formation of particles; hence, there is no time for the
particles to be aligned.
INTERNATIONAL JOURNAL OF FOOD PROPERTIES 2347

Figure 3. X-ray diffraction poster of coconut sugar powder particles produced by traditional method and drying methods.

100
90.5
90

80
71.4 70.9 70.9
69.25
70

60

50
%

40
30.75 29.1 29.1
28.6
30

20
9.5
10

0
Traditional Vacuum dried, Vacuum dried, Spray dried, C : Spray dried, C :
C : MD = 7 : 3 C : MD = 6 : 4 MD = 7 : 3 MD = 6 : 4
% Crystalline % Amorphous

Figure 4. Structural composition of coconut sugar powder produced by traditional method and drying methods.

Structural composition of coconut sugar samples is presented in Fig. 4. Traditional method


produced 90.5% crystalline and 9.5% amorphous structure. Amorphous structure of dried coconut
sugar powder ranged from 70.9% to 71.40% while crystalline state ranged from 28.6% to 30.75%.
Increase of maltodextrin concentration showed a slight increase in crystalline composition in coco-
nut sugar powder both in spray drying and in vacuum drying.
2348 B. NURHADI ET AL.

Vacuum drying method seemed to produce coconut sugar with more crystalline structure than
spray drying method. This might be due to the lower drying rate that allows crystallization to occur
compared to short drying process in spray drying. Vacuu- dried coconut sugar powder was ground
to create powder. Grinding or milling crystalline particles might reduce the total crystallinity 47

Hygroscopic rate
Figure 5 shows the hygroscopic rate of coconut sugar powder produced by traditional method and
drying methods. Increasing maltodextrin concentration reduces the rate of hygroscopicity in spray-
dried coconut sugar powder as shown in Figure. Same results were found with spray-dried sugar cane
powder 48, spray-dried grape syrup 49, and spray-dried acai powder 17, suggesting that maltodextrin
is an efficient drying aid in sugar-rich material spray drying process. This is due to the fact that
maltodextrin has the ability to decrease absorbed water by balancing the hydrophilic/hydrophobic
sites of powder particles and high glass transition temperature.50
Hygroscopic rate of spray dried coconut sugar powder is higher than vacuum dried coconut sugar
powder. Similar result was found in drying of passion fruit pulp powder and honey powder, spray-
dried powder resulted in higher water adsorption capacity than vacuum drying due to its spherical
particle shape which provides larger surface area.[19,36] Based on XRD analysis, increase in mal-
todextrin showed a less amount of amorphous structure that might impact its reactivity to surround-
ing moisture. More amorphous structure in powder is likely to cause more adsorption of water.
The traditional coconut sugar powder had the least hygroscopic rate, this might be due to its
higher crystalline structure. Properties of crystalline structure are non-hygroscopic, stable, and free-
flowing because crystalline structures are tightly packed so that water absorption only takes place on
the external surface of the crystal. Amorphous structures are haphazard, tangled, more open, and
porous; therefore, an individual molecule possesses more sites for external interaction, so amorphous
structure can absorb water easily.38 Some study also states that amorphous structure is more
hygroscopic because they have larger porosity and volume.51

Figure 5. Hygroscopic rate of coconut sugar powder produced by traditional method and drying methods.
INTERNATIONAL JOURNAL OF FOOD PROPERTIES 2349

100.00
93.00
88.08
90.00
80.17 82.86 82.79
80.00

70.00

60.00
L*

50.00

40.00

30.00
21.29 21.19
19.30
20.00 17.32
12.57
10.00
3.89 2.52 2.56 1.11 0.35
0.00
Traditional A (VD 7 : 3) B (VD 6 : 4) C (SD 7 : 3) D (SD 6 : 4)

Figure 6. L*, a*, and b* values of coconut sugar powder produced by traditional method and drying methods.

Colour
The colour parameters of coconut sugar powder are shown in Fig. 6. Traditional coconut sugar
powder showed low L* and high a* and b* values. Spray-dried coconut sugar powder shows a higher
value of L* than other methods. Furthermore, higher maltodextrin concentration also contributes to
higher L* value. The colour of vacuum-dried coconut sugar powder C : MD (7 : 3) and C : MD (6 :
4) seemed not different visually (Fig. 7). Higher a* values were shown by vacuum-dried coconut
sugar powder, while increasing maltodextrin concentration in spray drying will decrease a* value. A
slight difference was observed in b* value. The highest value of b* was shown by vacuum-dried C :
MD (7 : 3), followed by vacuum-dried C : MD (6 : 4), spray-dried C : MD (7 : 3), and spray-dried C :
MD (6 : 4). Increasing maltodextrin ratio may decrease b* value, meaning less yellow in colour.
Traditional coconut sugar powder appeared to be more red and yellow, less bright than vacuum
drying, while spray-dried sugar was vice versa. Brighter colour was obtained by using spray dryer
because the sample was converted into small droplets, hence the quicker the time for the particles to
dry.31 Since browning increases with time, it can be easily explained that the thicker samples took
more time to dry 52, which clarify the darker colours from vacuum-dried samples. Another

Figure 7. Coconut sugar powder produced by traditional method and drying methods.
2350 B. NURHADI ET AL.

Figure 8. Dissolving time of coconut sugar powder produced by traditional method and drying methods.

contributing factor to slightly darker colour is Maillard reaction, which happens between reducing
sugars and amino acids in foods which undergo thermal processing.53 Maillard reaction was strongly
affected by temperature, where browning reaction can increase alongside with increasing tempera-
ture. Traditional coconut sugar powder was produced using high temperature and exposed for a long
time, it caused a more dominant browning colour than those produced by drying methods.
Additionally, increasing maltodextrin will produce coconut sugar powder with a brighter colour,
with a decrease in redness and yellowness. Similar results have been reported in spray-dried coconut
sugar powder and foam-mat dried tamarind powder.[14,54]

Dissolving time
Crystalline structure would take more time to dissolve than amorphous structure 43 Traditional
coconut sugar powder tend to dissolve slowly because dissolution occurs only at the outer surface
exposed to the solvent. The particles are impermeable to the solvent because the molecules are
bonded tightly and density is high; therefore, the dissolution proceeds from outside to inside. In
contrast, amorphous powders particles are porous and hygroscopic and so they can dissolve
rapidly.38 Similar dissolving time was observed from vacuum-dried coconut sugar powder and
traditional (crystallized) coconut sugar (Fig. 8) . This could be explained that coconut sugar both
in crystallized and in amorphous forms composed mainly of sucrose having particle density higher
than water consequently sink easily when it poured to water and dissolve afterward.
From Figure 8, shorter dissolving time in vacuum drying is due to the different principles of
drying between spray dryer and vacuum drying, at which vacuum drying can result in larger
particles, more soluble and less dense than those obtained in conventional equipment, which led
to particles with lower moisture content and consequently lower water activity.55 The spray-dried
coconut sugar powder took the longest time to fully dispersed or completely dissolved in water. This
is due to more porous structure of spray-dried coconut sugar powder, hence less density compared
to those of vacuum dried. Less density impacted on low sink ability, which would further take effect
on longer dissolving time.[56,57] The result also showed that the dissolving time of coconut sugar
powder also increases with the increase of maltodextrin concentration in spray drying. Higher
maltodextrin concentration can lead to greater bulk density and particle size, which also related to
agglomeration process. Powder with high bulk density will be less porous and could be a contribut-
ing factor to reduction of water absorption.[14,50]
INTERNATIONAL JOURNAL OF FOOD PROPERTIES 2351

Figure 9. Powder recovery of coconut sugar powder produced by traditional method and drying methods.

Powder recovery
Powder recovery of coconut sugar powder is affected by drying methods as shown in Fig. 9. Vacuum-
dried coconut sugar powder resulted in higher powder recovery than that of spray drying. Spray drying
can produce fine dry particles by atomizing sample into small droplets and blown by hot air, the droplet
will dry quickly, and the dried particles will fall into the lower part of the dryer. 31 Despite its speed to dry
samples, powder can stick onto the drying chamber during spray drying, resulting in smaller powder
recovery and operational problems, caused by high adhesiveness and hygroscopicity.[58,59] While the
drying rate in vacuum drying was lower compared to spray drying, evaporation of water occurs at low
oxygen pressure, resulting in a smaller chance of oxidative degradation, e.g., enzymatic browning caused
by the oxidation process in the final product. Vacuum condition can cause water to boil, thus creating a
porous structure that helps to remove moisture quickly while drying. 10
Powder recovery of traditionally produced coconut sugar powder has a higher value than
vacuum-dried and spray-dried coconut sugar powder. Traditionally produced coconut sugar powder
is made by the slow crystallization of sucrose because of low rate of water evaporation from the sap
until it becomes oversaturated.60 This condition caused a co-crystallization in sugar and turns the
particles in coconut sugar powder into crystalline form.61 This high amount of crystalline particle in
traditionally produced coconut sugar powder makes them more stable. Thus, the instantaneous
process of stickiness in the amorphous sugar because of plasticization of particle surfaces which
allows a sufficient decrease of surface viscosity for the formation of liquid bridges between particles
does not occur.62 Because of it, traditionally produced coconut sugar powder has the highest powder
recovery among the others with the value nearly reaching 100%. Sugarcane processing into crystals
was made by adding calcium carbonate, yielding 96 to 98% sucrose. 38
A higher result of powder recovery is obtained with increasing maltodextrin concentration by
using spray drying and vacuum drying. Increasing maltodextrin will also create a higher content of
total solids in the solution, it would produce more density, meaning higher viscosity; this condition
could lead to lower values of radial speed of spray drying and will reduce the intensity and speed of
droplets colliding with the internal wall of the drying chamber, thus more powder is recovered and
lesser deposits in the chamber.48 Addition of maltodextrin into coconut sap solution will increase
Tg, hence reducing stickiness by balancing hydrophilic and hydrophobic sites of sugar powder. This
condition will reduce the amount of absorbed water in which hydrogen bond in the water molecule
2352 B. NURHADI ET AL.

and hydroxyl in the amorphous and crystalline structure are responsible.59 More powder recovery is
also obtained with increasing maltodextrin concentration in spray-dried coconut sap, sucrose, honey,
and concentrated fruit juices.[45,58] Substituting maltodextrin with whey protein isolate could also
increase powder recovery of spray dried coconut sugar powder from 39.39–54.42% up to 67.82%–
72.55% (data not shown).

Conclusion
Coconut sugar powder was produced using traditional and drying methods (spray drying and
vacuum drying) by addition of drying aid in the form of maltodextrin. Traditional coconut sugar
powder has a dominant crystalline structure while dried ones have amorphous structure. Traditional
coconut sugar powder had a dominant crystalline structure (90.5%), with lowest monolayer moisture
content, hygroscopic rate, L* and highest a* and b* values compared to drying methods. The drying
methods (vacuum and spray drying) produced coconut sugar powder successfully with properties
different from sugar obtained by using traditional method. Increasing maltodextrin would increase
the stability of coconut sugar powder obtained indicated by higher monolayer moisture content, low
higroscopic rate, and low amorphous content. This study offers a better understanding of crystalline
and amorphous coconut sugar characteristics which is produced by adifferent method. Such
information can be used as an alternative process to produce coconut sugar powder with desired
properties.

Funding
This work was supported by the Universitas Padjadjaran.

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